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Title: Effect of Ni particle size on the production of renewable methane from CO2 over Ni/CeO2 catalyst

Abstract

Production of ‘renewable Methane’ has attracted renewed research interest as a fundamental probe reaction and process for CO2 utilization through potential use in C1 fuel production and even for future space exploration technologies. CO2 methanation is a structure sensitive reaction on Ni/CeO2 catalysts. To precisely elucidate the size effect of the Ni metal center on the CO2 methanation performance, we prepared 2%Ni/CeO2 catalysts with pre-synthesized uniform Ni particles (2, 4 and 8 nm) on a high surface area CeO2 support. Transmission electron microscopy (TEM) and ambient pressure X-ray photo spectroscopy (AP-XPS) characterization have confirmed that the catalyst structure and chemical state was uniform and stable under reaction conditions. The 8 nm sized catalyst showed superior methanation selectivity over the 4 and 2 nm counterparts, and the methanation activity in term of TOF is 10 times and 70 times higher than for the 4 and 2 nm counterparts, respectively. Here, the DRIFTS studies revealed that the larger Ni (8 nm particles) over CeO2 efficiently facilitated the hydrogenation of the surface formate intermediates, which is proposed as the rate determining step accounting for the excellent CO2 methanation performance.

Authors:
 [1];  [2];  [3]; ORCiD logo [4];  [5];  [2];  [6];  [2];  [3];  [6]; ORCiD logo [7];  [8]; ORCiD logo [2]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States); Zhejiang Univ. of Technology (China)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Univ. of Virginia, Charlottesville, VA (United States)
  4. Univ. Politècnica de Catalunya, Barcelona (Spain)
  5. Zhejiang Univ. (China)
  6. State Univ. of New York, Stony Brook, NY (United States)
  7. Univ. of Pennsylvania, Philadelphia, PA (United States)
  8. Brookhaven National Lab. (BNL), Upton, NY (United States); State Univ. of New York, Stony Brook, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1798484
Alternate Identifier(s):
OSTI ID: 1782376
Report Number(s):
BNL-221683-2021-JAAM
Journal ID: ISSN 2095-4956
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Energy Chemistry
Additional Journal Information:
Journal Volume: 61; Journal ID: ISSN 2095-4956
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Lin, Lili, Gerlak, Clifford A., Liu, Chang, Llorca, Jordi, Yao, Siyu, Rui, Ning, Zhang, Feng, Liu, Zongyuan, Zhang, Sen, Deng, Kaixi, Murray, Christopher B., Rodriguez, José A., and Senanayake, Sanjaya D. Effect of Ni particle size on the production of renewable methane from CO2 over Ni/CeO2 catalyst. United States: N. p., 2021. Web. doi:10.1016/j.jechem.2021.02.021.
Lin, Lili, Gerlak, Clifford A., Liu, Chang, Llorca, Jordi, Yao, Siyu, Rui, Ning, Zhang, Feng, Liu, Zongyuan, Zhang, Sen, Deng, Kaixi, Murray, Christopher B., Rodriguez, José A., & Senanayake, Sanjaya D. Effect of Ni particle size on the production of renewable methane from CO2 over Ni/CeO2 catalyst. United States. https://doi.org/10.1016/j.jechem.2021.02.021
Lin, Lili, Gerlak, Clifford A., Liu, Chang, Llorca, Jordi, Yao, Siyu, Rui, Ning, Zhang, Feng, Liu, Zongyuan, Zhang, Sen, Deng, Kaixi, Murray, Christopher B., Rodriguez, José A., and Senanayake, Sanjaya D. Wed . "Effect of Ni particle size on the production of renewable methane from CO2 over Ni/CeO2 catalyst". United States. https://doi.org/10.1016/j.jechem.2021.02.021. https://www.osti.gov/servlets/purl/1798484.
@article{osti_1798484,
title = {Effect of Ni particle size on the production of renewable methane from CO2 over Ni/CeO2 catalyst},
author = {Lin, Lili and Gerlak, Clifford A. and Liu, Chang and Llorca, Jordi and Yao, Siyu and Rui, Ning and Zhang, Feng and Liu, Zongyuan and Zhang, Sen and Deng, Kaixi and Murray, Christopher B. and Rodriguez, José A. and Senanayake, Sanjaya D.},
abstractNote = {Production of ‘renewable Methane’ has attracted renewed research interest as a fundamental probe reaction and process for CO2 utilization through potential use in C1 fuel production and even for future space exploration technologies. CO2 methanation is a structure sensitive reaction on Ni/CeO2 catalysts. To precisely elucidate the size effect of the Ni metal center on the CO2 methanation performance, we prepared 2%Ni/CeO2 catalysts with pre-synthesized uniform Ni particles (2, 4 and 8 nm) on a high surface area CeO2 support. Transmission electron microscopy (TEM) and ambient pressure X-ray photo spectroscopy (AP-XPS) characterization have confirmed that the catalyst structure and chemical state was uniform and stable under reaction conditions. The 8 nm sized catalyst showed superior methanation selectivity over the 4 and 2 nm counterparts, and the methanation activity in term of TOF is 10 times and 70 times higher than for the 4 and 2 nm counterparts, respectively. Here, the DRIFTS studies revealed that the larger Ni (8 nm particles) over CeO2 efficiently facilitated the hydrogenation of the surface formate intermediates, which is proposed as the rate determining step accounting for the excellent CO2 methanation performance.},
doi = {10.1016/j.jechem.2021.02.021},
journal = {Journal of Energy Chemistry},
number = ,
volume = 61,
place = {United States},
year = {Wed Mar 10 00:00:00 EST 2021},
month = {Wed Mar 10 00:00:00 EST 2021}
}

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